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响应化学燃料的时空可用性,从稳定聚集体到耗散聚集体的瞬态转变

Transient transition from Stable to Dissipative Assemblies in Response to the Spatiotemporal Availability of a Chemical Fuel.

作者信息

Kar Haridas, Chen Rui, Das Krishnendu, Prins Leonard J

机构信息

Department of Chemical Sciences, University of Padua, Via Marzolo 1, 35131, Padua, Italy.

出版信息

Angew Chem Int Ed Engl. 2025 Jan 10;64(2):e202414495. doi: 10.1002/anie.202414495. Epub 2024 Nov 11.

Abstract

The transition from inactive to active matter implies a transition from thermodynamically stable to energy-dissipating structures. Here, we show how the spatiotemporal availability of a chemical fuel causes a thermodynamically stable self-assembled structure to transiently pass to an energy-dissipating state. The system relies on the local injection of a weak affinity phosphodiester substrate into an agarose hydrogel containing surfactant-based structures templated by ATP. Injection of substrate leads to the inclusion of additional surfactant molecules in the assemblies leading to the formation of catalytic hotspots for substrate conversion. After the local disappearance of the substrate as a result of chemical conversion and diffusion the assemblies spontaneously return to the stable state, which can be reactivated upon the injection of a new batch of fuel. The study illustrates how a dissipating self-assembled system can cope with the intermittent availability of chemical energy without compromising long-term structural stability.

摘要

从非活性物质到活性物质的转变意味着从热力学稳定结构到能量耗散结构的转变。在此,我们展示了化学燃料的时空可用性如何使热力学稳定的自组装结构短暂地转变为能量耗散状态。该系统依赖于将弱亲和力的磷酸二酯底物局部注入到含有由ATP模板化的基于表面活性剂的结构的琼脂糖水凝胶中。底物的注入导致组装体中包含额外的表面活性剂分子,从而形成用于底物转化的催化热点。由于化学转化和扩散导致底物局部消失后,组装体自发地恢复到稳定状态,在注入新一批燃料后可重新激活。该研究说明了一个耗散性自组装系统如何在不损害长期结构稳定性的情况下应对化学能的间歇性可用性。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/0e23/11720371/fd5d914551ad/ANIE-64-e202414495-g003.jpg

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